ENERGY & FUELS
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2020
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IF 3.421
Shiwei Ma,Shiyi Chen,Huijun Ge,Tao Song,Ping Lu,Wenguo Xiang
CeO2 is a typical fluorite oxide with desirable lattice oxygen conductivity and can be applied as an active support for the Fe-based oxygen carrier in chemical looping hydrogen generation (CLHG). However, Fe2O3/CeO2 always suffers from low thermal stability and sintering. Doping foreign cations could be a proper way to improve its reactivity and cyclic stability. In this work, Zr4+ and Sm3+, with a smaller ionic radius and lower valence than Ce4+, respectively, were doped into Fe2O3/CeO2 using the co-precipitation method, and the doping effects on the reactivity and redox stability of Fe2O3/CeO2 in CLHG were investigated. Fe2O3/Ce0.6Sm0.15Zr0.25O1.925 provided the best redox reactivity, and the purity of generated hydrogen for all oxygen carriers reached nearly 100% (the detection limit of CO/CO2 was 0.01% in volume). The reactivity followed the sequence Fe2O3/Ce0.6Sm0.15Zr0.25O1.925 > Fe2O3/Ce0.8Sm0.2O1.9 > Fe2O3/Ce0.75Zr0.25O2 > Fe2O3/CeO2. However, the concentration of oxygen vacancy was ranked as Fe2O3/Ce0.8Sm0.2O1.9 > Fe2O3/Ce0.6Sm0.15Zr0.25O1.925 > Fe2O3/Ce0.75Zr0.25O2 > Fe2O3/CeO2. The Zr doping boosted the reactivity of Fe2O3/CeO2 mainly by enhancing its sintering resistance, whereas the Sm doping achieved it mainly by promoting the oxygen conductivity, whose ability to improve the thermal stability of Fe2O3/CeO2 was rather limited. Both Zr and Sm doping could suppress the outward migration of Fe cations in the particles, resulting in higher sintering resistance. Furthermore, Zr and Sm could dissolve into CeO2 for prepared Fe2O3/Ce0.6Sm0.15Zr0.25O1.925; however, the bleeding out of both dopants was observed with Sm0.5Zr0.5O1.75 formation, which could be detrimental to the redox stability of the oxygen carrier.
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DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
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2025
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IF 13.2
Jia-Hui Chen,Hao-Yu Jiang,Wen-Qiang Gong,Wei Hui,Xiao-Liang Zhang,Ming-Shuai Sun,Jia-Yin Zhang,Dan-Dan Cai,Duan-Jian Tao
Metal-organic frameworks (MOFs) have been acclaimed as potential adsorbents for gas separation, yet their intrinsic microporosity and site-saturated coordination often lead to slow adsorption kinetics and poor selectivity under low-concentration gas conditions. To address this challenge, we developed an acetic acid-assisted synthesis strategy to engineer Zr-based MOFs (UiO-66-V, V = acetic acid volume) with enhanced Lewis acids sites and porous structure. The optimal UiO-66-2.5 variant achieves an adsorption rate six times higher than that of pristine UiO-66 and superior ideal adsorption solution theory selectivities for 3 % NH 3 /97 % N 2 (745) and 3 % NH 3 /97 % H 2 (6036) at 298.2 K and 1.0 bar. Dynamic breakthrough experiments confirm the excellent regenerative stability and separation performance of UiO-66-2.5, achieving a retention time of 120 min g −1 for a simulated industrial gas mixture (3 % NH 3 /24.25 % N 2 /72.75 % H 2 ), outperforming pristine UiO-66 (84 min g −1 ). Furthermore, the optimized 90 % UiO-66-2.5@PVA pellets exhibit a breakthrough time of 100 min·g −1 , which is comparable to that of the UiO-66-2.5 powder. Moreover, UiO-66-2.5 could maintain 92 % capacity over 10 adsorption-regeneration cycles. Comprehensive characterization studies revealed that the enhanced NH 3 uptake and separation performance originate from the higher surface areas and increased Lewis acids sites in UiO-66-2.5 compared to the pristine material. This work establishes acid-assisted synthesis as an effective strategy for designing MOFs that meet the capacity, kinetics, and stability requirements for industrial NH 3 capture.
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DOI
高影响因子
APPLIED CATALYSIS A-GENERAL
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2025
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IF 4.8
Zhenhui Huang,Xiangying Wang,Wei Na,Xinyu Ling,Xingpeng Sun,Runqin Chen,Wengui Gao,Hua Wang
The surface properties of catalysts play a crucial role in CO 2 hydrogenation. In this study, Cu-loaded Ce–Zr oxide (CCZ) catalysts with distinct activities were synthesized via four methods. Catalytic testing revealed that the CCZ-HM catalyst exhibited the highest performance, achieving the greatest methanol space–time yield (STY). Structural and surface analyses revealed that low-valence Cu specie, oxygen vacancies, strong metal–support interactions, and balanced acid–base properties contributed to enhanced catalytic performance of the CCZ catalysts. Mechanistic studies indicated that CCZ-CP and CCZ-HM catalysts exhibited higher oxygen vacancy concentrations and enhanced surface acidity-basicity, which promoted CO₂ adsorption and the formation of carbonate species. In a CO 2 + H 2 atmosphere, both catalysts mainly formed bidentate formate species, which served as key intermediates in methanol synthesis. However, the strong adsorption capacity and limited H 2 spillover of the CCZ-CP catalyst hindered further hydrogenation of these intermediates, thereby reducing methanol production. In contrast, the excellent acid–base synergy and efficient H₂ spillover of CCZ-HM promoted the hydrogenation of CO₂-derived intermediates to methanol, resulting in enhanced STY. These findings indicate that the rational control of catalyst surface acidity, oxygen vacancy concentration, and H 2 activation ability is crucial for improving overall catalyst performance.
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DOI
高影响因子
ACS Applied Materials & Interfaces
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2022
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IF 10.383
Qinong Shao,Chenhui Yan,Mingxi Gao,Wubin Du,Jian Chen,Yaxiong Yang,Jiantuo Gan,Zhijun Wu,Wenping Sun,Yinzhu Jiang,Yongfeng Liu,Mingxia Gao,Hongge Pan
Halide solid electrolytes have been considered as the most promising candidates for practical high-voltage all-solid-state lithium-ion batteries (ASSLIBs) due to their moderate ionic conductivity and good interfacial compatibility with oxide cathode materials. Aliovalent ion doping is an effective strategy to increase the ionic conductivity of halide electrolytes. However, the effects of ion doping on the electrochemical stability window of halide electrolytes and carbon additive on electrochemical performance are still unclear by far. Herein, a series of Zr-doped Li3–xEr1–xZrxCl6 halide solid electrolytes (SEs) are synthesized through a mechanochemical method and the effects of Zr substitution on the ionic conductivity and electrochemical stability window are systematically investigated. Zr doping can increase the ionic conductivity, whereas it narrows the electrochemical stability window of the Li3ErCl6 electrolyte simultaneously. The optimized Li2.6Er0.6Zr0.4Cl6 electrolyte exhibits both a high ionic conductivity of 1.13 mS cm–1 and a high oxidation voltage of 4.21 V. Furthermore, carbon additives are demonstrated to be beneficial for achieving high discharge capacity and better cycling stability and rate performance for halide-based ASSLIBs, which are completely different from the case of sulfide electrolytes. ASSLIBs with uncoated LiCoO2 cathode and carbon additives exhibit a high discharge capacity of 147.5 mAh g–1 and superior cycling stability with a capacity retention of 77% after 500 cycles. This work provides an in-depth understanding of the influence of ion doping and carbon additives on halide solid electrolytes and feasible strategies to realize high-energy-density ASSLIBs.
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DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
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2023
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IF 15.1
Xiaobo Bai,Chengyan Liu,Fucong Li,Zhongwei Zhang,Ying Peng,Ruifan Si,Baoquan Feng,Guojing Wu,Jie Gao,Haiqiao Wei,Lei Miao
Lead-free GeTe-based thermoelectric (TE) materials are most promising candidates to replace the environmentally harmful PbTe for TE application at middle temperature range, where high power factor ( PF ) is significantly important for high power generation if the cost of heat source is low enough. In this study, we report for the first time that the PF of GeTe can be greatly enhanced by tailoring the interaction between Te 5s 2 lone pair and antibonding orbitals, which is induced by the hybridization of Zr 4d 2 electrons with antibonding orbitals. As a result, the contribution of Ge 4s 2 electrons to the valence band is promoted, leading to the band sharpening at the valence band maximum in rhombohedral phase, and simultaneous band sharpening at the valence band maximum and band flattening at the conduction band minimum in cubic phase. Lower band effective mass m b * effectively increases the carrier mobility to a very high value of ∼121 cm −2 V −1 s −1 (300 K), and the Seebeck coefficient is improved by the reduced detrimental effect of minority carrier in cubic phase, enhancing the maximum PF up to a record value of ∼5503 μW m −1 K −1 . With the assistance of reduced thermal conductivity, a peak zT of ∼1.9 is achieved at 673 K, which is one of the highest values among single doped GeTe. This work provides a new guidance to enhance the TE performance of GeTe-based materials.
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DOI
高影响因子
COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
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2021
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IF 4.539
Bohao Yang,Mingbo Shi,Renliang Huang,Wei Qi,Rongxin Su,Zhimin He
The treatment of oil spill and the separation of oil-water mixture have been widely concerned in recent years. In this work, a one-pot synthesis strategy is developed to prepare fluorine functionalized zirconium-based metal organic framework (Zr-MOFs) (denoted as UiO-66-1F) by using 4-fluorobenzoic acid as modulator and modifier and p-phthalic acid (PTA) as ligand. 4-fluorobenzoic acid can participate in the formation of frameworks structure and cause structural defects, causing larger surface area and hierarchically porous structure. The hydrophobicity of UiO-66-1F increases with increasing of the ratio of 4-fluorobenzoic acid to zirconium chloride and when the ratio is 10, the synthesized UiO-66-1F(10) shows high hydrophobicity with a water contact angle (WCA) of 122° while the WCA of original UiO-66 is only 21°. UiO-66-1F(10) also has good chemical stability over a wide pH range (pH 1∼11) and good hydrothermal stability. In addition, a superhydrophobic sponge (UiO-66-1F(10)@PDA@sponge) with a WCA of 150° was prepared via in situ growth of UiO-66-1F(10) on a polydopamine modified sponge (PDA@sponge). The resulting composite shows high absorption capacities for various oils and organic solvents ranging from 50.5 g/g (n-hexane)– 107.8 g/g (dichloromethane) and good recyclability.
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DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
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2019
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IF 8.355
Zhen Huang,Minghu Zhao,Chen Wang,Shixing Wang,Linqing Dai,Libo Zhang,Lei Xu
A novel metal organic framework absorbent was synthesized by one step method using 2,2′-dithiodibenzoic acid as organic linker for efficient and selective recovery of Au(III) from aqueous solution. The adsorbent were detected by scanning electron microscope, X-ray diffraction and zeta potential instruments. Its performance was tested by batch experiments. The adsorption isotherm conforms to the Langmuir model, demonstrating that the adsorption process is the uniform monolayer adsorption. The kinetic model is well fitted to the pseudo second-order dynamics model. The maximum adsorption capacity was 1119 mg/g at pH = 2. High temperatures can promote the absorption process. The five adsorption and desorption cycles indicate that the adsorbent has good repeatability for Au(III) adsorption. It could selectively adsorbed Au(III) from wastewater. The adsorption derive from chelation and reduction. The DFT and XPS results show that Au(III) is mainly adsorbed on the adsorbent by coupling with the S atom. These results indicate that it has a high potential to remove Au(III) from industrial wastewater.
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高影响因子
CERAMICS INTERNATIONAL
·
2024
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IF 5.1
Chao Li,Ying Li,Yi Xu,Jiyou Zhong
Near-infrared (NIR) phosphors as crucial components of NIR light sources have multifunctional and smart spectroscopy applications, prompting an increasing research interest in developing efficient and stable NIR materials. Focusing on this issue, the present study explored the luminescent properties of Cr 3+ -doped Ca 3 ZnMGe 3 O 12 (M = Zr, Hf, Sn and Ti) garnet family. These materials exhibit an emission peak falls within the range of 785–805 nm with a full width at half maximum (FWHM) varying from 114 to 123 nm. Among them, the Ca 3 ZnZrGe 3 O 12 :Cr 3+ phosphor shows the highest photoluminescence quantum yield (PLQY = 60.3 %) and an excellent thermal stability ( I 423K / I 298K = 77.51 %). Moreover, the performance of a prototype Ca 3 ZnZrGe 3 O 12 :Cr 3+ -containing NIR pc-LED device was estimated, which achieves an NIR output of 23.46 mW and a photonic efficiency of 14.09 % under 100 mA driving current. Non-destructive examination can be realized using this light source, demonstrating the good potential of the material in NIR spectroscopy applications.
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DOI
高影响因子
Journal of Environmental Sciences
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2025
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IF 6.3
Rui Ma,Xinjie Cui,Youyi Liu,Qianhui Xu,Weiwei Wang,Guangze Nie
Nanocomposites fabricated through the encapsulation of hydrated Zr(IV) oxide (HZO) nanoparticles within millimeter-scale hosts have emerged as promising candidates for phosphate sequestration from water. However, achieving ultrasmall nanoparticles within these hosts that maintain high decontamination reactivity is still a significant challenge. Herein, a novel nanocomposite (denoted HZO@CS-PEI) was obtained by confining the growth of HZO in dual crosslinked network hydrogels composed of interpenetrating chitosan (CS) and polyethyleneimine (PEI). Benefiting from the confinement effect of the dual cross-linked structure, the HZO within HZO@CS-PEI exhibited an ultrasmall size of approximately 2.16 nm. The incorporation of PEI enhanced both phosphate sequestration efficiency and mechanical stability of the nanocomposite, improving its practical applicability. Ultrafine dispersion of HZO nanoparticles within the composite matrix achieved a saturable phosphate adsorption capacity exceeding 64.41 mg/g at 298 K. Crucially, selective phosphate adsorption by HZO@CS-PEI remained effective in water containing high concentrations of coexisting anions and organic matter. The synergistic application of spectroscopic analyses and density functional theory (DFT) calculations revealed three distinct interaction mechanisms between HZO@CS-PEI and phosphate: inner-sphere complexation, hydrogen bonding, and electrostatic interactions. Furthermore, the used HZO@CS-PEI could be effectively regenerated with 0.1 mol/L NaOH for repeat use. In the column adsorption tests, phosphate-contaminated water was successfully treated by HZO@CS-PEI columns over 2750 bed volumes (BV), confirming operational stability under dynamic flow conditions.
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高影响因子
ACS Applied Nano Materials
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2025
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IF 5.5
Jing Chen,Jiawen Li,Huanhuan Wang,Xincun Dou,Baiyi Zu
How to modulate the open metal sites (OMS) for enhancing the luminescence emerges as a significant issue to explore in the exploration of high-performance metal-organic frameworks (MOFs) for photoluminescence (PL) sensing and X-ray detection. Here, by efficiently extending the conjugation of the ligand, nanoscale Zr-ADIP, which has eight OMS per Zr cluster, was first synthesized and demonstrated to have enhanced PL and X-ray excited luminescence (XEL) performance. Furthermore, a modulator tuning strategy was adopted to occupy the OMS, which has been proven to be efficient for engineering the unoccupied electronic levels, promoting the relaxation of the excited electrons, and enhancing the PL efficiency. It is found that with benzoic acid as the modulator, the optimal nanoscale Zr-ADIP-BzOH exhibits superior performance with an X-ray detection limit of 0.53 μGy s–1, which is 10 times lower than the minimum X-ray dose rate requirement for medical X-ray imaging. The superior XEL performance of Zr-ADIP-BzOH has been further proven to be effective in the tentative monitoring of the morphology of a mature pearl in a clam sample by constructing a condensed film device. We expect that the proposed OMS introduction and modulator tuning strategy would offer insights for the structural design and performance enhancement of luminescent MOFs.
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高影响因子
SURFACE & COATINGS TECHNOLOGY
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2025
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IF 6.1
Xiaona Ren,Zhipei Chen,Peng Wang,Wenchang Wang,Yao Wang,Changchun Ge
Rare earth oxide (CeO₂/Y₂O₃) reinforced AlCrFeNiCu high-entropy alloy coatings with a Mo interlayer (designated as Mo/CeO₂-AlCrFeNiCu and Mo/Y₂O₃-AlCrFeNiCu) were successfully deposited onto a Zr-4 substrate via high-speed laser cladding. The microstructural characteristics and properties of the composite coatings were comprehensively investigated. The results demonstrate that the Mo interlayer alleviates the thermal mismatch between the substrate and the HEA coatings and, to a certain degree, counteracts the grain refinement effect induced by the rare earth oxides. Overall, it plays a critical role in enhancing interfacial structural stability, mitigating thermal stress, and improving overall coating performance. It effectively optimizes the coating-substrate bonding integrity, reduces susceptibility to high-temperature fretting fatigue and plastic deformation, and significantly lowers the specific wear rate. Furthermore, the Mo interlayer enhances the compactness and continuity of the interface, suppresses the formation of corrosive pathways, and promotes the formation of a thicker, more stable passive film on the coating surface.
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产品关联
DOI
高影响因子
CERAMICS INTERNATIONAL
·
2020
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IF 3.83
Mingxue Wang,Kun Wang,Xiaobing Huang,Tao Zhou,Huasheng Xie,Yurong Ren
To improve the intrinsic electronic conductivity of Na 3 V 2 (PO 4 ) 2 F 3 (NVPF), zirconium (Zr) was introduced into the NVPF/C compound through a carbothermal reduction reaction with citric acid as the carbon source. The effects of Zr 4+ doping on the crystal structure and morphology of the as-prepared materials were analyzed. Electrochemical and kinetic properties of the samples were investigated by galvanostatic charge-discharge, CV and EIS test. It is confirmed that moderate Zr 4+ doping can improve the electrochemical performance of NVPF. Among all Na 3 V 2-x Zr x (PO 4 ) 2 F 3 /C (x = 0, 0.01, 0.05, 0.1) samples, Na 3 V 1·95 Zr 0·05 (PO 4 ) 2 F 3 /C shows the best rate and cycle performance. It exhibits the highest specific capacity of 121.8 and 110.3 mAh/g at 0.2 and 10 C, respectively, and maintains a capacity retention of approximately 83.6% after 1000 cycles at 5 C. The kinetic properties results show that the excellent electrochemical performance of Na 3 V 1·95 Zr 0·05 (PO 4 ) 2 F 3 /C can be attributed to the increase in electronic conductivity and ion diffusion coefficient .
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DOI
高影响因子
危险品化学品经营许可证（带存储）